Determination of alpha dose rate profile at the HLW nuclear glass/water interface h i g h l i g h t s

International audienceThe nuclear glass/water interface is studied. The way the energy of alpha particles is deposited is modeled using MCNPX code. A model giving dose rate profiles at the interface using intrinsic data is proposed. Bulk dose rate is a majoring estimation in alteration layer and in surrounding water. Dose rate is high in small cracks; in larger ones irradiated volume is negligible. a b s t r a c t Alpha irradiation and radiolysis can affect the alteration behavior of High Level Waste (HLW) nuclear glasses. In this study, the way the energy of alpha particles, emitted by a typical HLW glass, is deposited in water at the glass/water interface is investigated, with the aim of better characterizing the dose deposition at the glass/water interface during water-induced leaching mechanisms. A simplified chemical composition was considered for the nuclear glass under study, wherein the dose rate is about 140 Gy/h. The MCNPX calculation code was used to calculate alpha dose rate and alpha particle flux profiles at the glass/water interface in different systems: a single glass grain in water, a glass powder in water and a water-filled ideal crack in a glass package. Dose rate decreases within glass and in water as distance to the center of the grain increases. A general model has been proposed to fit a dose rate profile in water and in glass from values for dose rate in glass bulk, alpha range in water and linear energy transfer considerations. The glass powder simulation showed that there was systematic overlapping of radiation fields for neighboring glass grains, but the water dose rate always remained lower than the bulk value. Finally, for typical ideal cracks in a glass matrix, an overlapping of irradiation fields was observed while the crack aperture was lower than twice the alpha range in water. This led to significant values for the alpha dose rate within the crack volume, as long as the aperture remained lower than 60 lm

Alpha dose rate and decay dose impacts on the long-term alteration of HLW nuclear glasses

International audienceIn the prospect of deep geological disposal, the long-term behavior of high-level nuclear glasses has to be investigated regarding alpha radiation induced by long-life minor actinides. The present study focuses on the effects of alpha radiation on the long-term chemical reactivity of R7T7-type glasses, by separately considering the alpha dose rate and the alpha decay dose. Old SON68 glasses doped with 238/239PuO2 or 244CmO2 were studied to simulate high alpha dose rates corresponding to an early water ingress and a high level of alpha decay doses corresponding to long-term disposal conditions. A part of the 238/239Pu-doped glass block was annealed to fully recover the irradiation-induced damage accumulated since the glass was fabricated and to dissociate the effect of the alpha dose rate from that of the alpha decay dose. The glasses were then leached under static conditions at 90 °C for several years. The results showed that the residual alteration rate is not affected by the alpha dose rate over a wide range of dose rate values expected under disposal conditions: this glass remained relatively insensitive to the alpha radiolysis phenomena at the glass - water interface. However, over the duration of the experiments, the residual alteration rate of the damaged 238/239Pu-doped glass was enhanced compared to that of the annealed glass (Figure 1). This result, underlying the role of the damaged glass structure on its macroscopic behavior, is in agreement with those obtained on previous studies on a 244Cm-doped glass [1] and with leaching behavior of simplified externally irradiated glasses [2-3], indicating that the ballistic effects of the recoil nuclei are responsible for this increase in the residual alteration rate

Heavy ion radiation ageing impact on long-term glass alteration behavior

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Atom-Probe Tomography, TEM and ToF-SIMS study of borosilicate glass alteration rim: A multiscale approach to investigating rate-limiting mechanisms

International audienceSignificant efforts have been made into understanding the dissolution of silicate glasses and minerals, but there is still debate about the formation processes and the properties of surface layers. Here, we investigate glass coupons of ISG glass – a 6 oxide borosilicate glass of nuclear interest – altered at 90 °C in conditions close to saturation and for durations ranging from 1 to 875 days. Altered glass coupons were characterized from atomic to macroscopic levels to better understand how surface layers become protective. With this approach, it was shown that a rough interface, whose physical characteristics have been modeled, formed in a few days and then propagated into the pristine material at a rate controlled by the reactive transport of water within the growing alteration layer. Several observations such as stiff interfacial B, Na, and Ca profiles and damped profiles within the rest of the alteration layer are not consistent with the classical inter-diffusion model, or with the interfacial dissolution-precipitation model. A new paradigm is proposed to explain these features. Inter-diffusion, a process based on water ingress into the glass and ion-exchange, may only explain the formation of the rough interface in the early stage of glass corrosion. A thin layer of altered glass is formed by this process, and as the layer grows, the accessibility of water to the reactive interface becomes rate-limiting. As a consequence, only the most easily accessible species are dissolved. The others remain undissolved in the alteration layer, probably fixed in highly hydrolysis resistant clusters. A new estimation of water diffusivity in the glass when covered by the passivating layer was determined from the shift between B and H profiles, and was 10−23 m2.s−1, i.e. approximately 3 orders of magnitude lower than water diffusivity in the pristine material. Overall, in the absence of secondary crystalline phases that could consume the major components of the alteration layer (Si, Al), it is assumed that the glass dissolution rate continuously decreases due to the growth of the transport limiting alteration layer, in good agreement with residual rates reported in the literature for this glass. According to our results it can be expected that new kinetic models should emerge from an accurate time dependent budget of water within the nanoporous alteration layer